Development and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-Based CO2 and SO32– and SO42– Loaded Capture Process Solutions via FT-IR Spectroscopy

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avondale-bepress-to-dspace.facultyScience
avondale-bepress-to-dspace.peer_review_statusPeer reviewed before publication
avondale-bepress.abstract<p>CO<sub>2</sub> capture using aqueous ammonia is a potentially attractive option for emissions reductions from energy production and industrial processes. From an operational perspective, the capture absorbent must be monitored continuously to maintain the maximum efficiency of the capture process. In practice the composition of the absorbent is typically evaluated offline and retrospectively via wet chemistry methods, delaying any necessary variations to the process conditions to maintain maximum efficiency. Online absorbent monitoring methods incorporating spectroscopy via Raman or Fourier transform infrared (FT-IR) are attractive options due to their rapid response times and flexibility of the resulting output to be incorporated directly into process control packages. The present study outlines an evaluation of the FT-IR spectroscopic technique with analysis via partial least squares regression (PLSR) for a range of dilute to concentrated aqueous ammonia absorbents from ∼0.3–6.0 M and over a range of CO<sub>2</sub> loadings from ∼0.0–0.6 mol CO<sub>2</sub>/mol NH<sub>3</sub>. The water concentration in the samples ranges from ∼35.2–55.2 M. The effect of interfering SO<sub><em>x</em></sub> species on the FT-IR method has been evaluated by incorporating dissolved SO<sub>3</sub><sup>2–</sup> and SO<sub>4</sub><sup>2–</sup> components into the solutions from 0.0–1.5 M. The analysis results in accurate concentrations for all analytes. The robustness of the analysis results has been evaluated and discussed. Additionally, FT-IR spectroscopy with PLSR was compared with conventional titration methods for a selected series of mixed NH<sub>3</sub>/CO<sub>2</sub> standard solutions and a series of liquid samples from a bench-scale CO<sub>2</sub> absorption process. At low concentrations where the total NH<sub>3</sub> concentration is less than 4.0 M and the total CO<sub>2</sub> concentration is less than 1.5 M, both the combined PLSR with FT-IR method and the conventional potentiometric titration methods were suitable for the evaluation of the liquid compositions. However, at concentrations out of the low concentration range, the combined PLSR and FT-IR method was proven to have a robustness and accuracy greater than those of the conventional potentiometric titration methods. Therefore, given the simplicity and rapid turnaround of FT-IR spectroscopy in combination with PLSR, we consider this to be a superior and flexible technique for monitoring of CO<sub>2</sub> loaded aqueous ammonia solutions.</p>
avondale-bepress.articleid1092
avondale-bepress.authorsLichun Li
avondale-bepress.authorsRobert Bennett
avondale-bepress.authorsWilliam Conway
avondale-bepress.authorsHai Yu
avondale-bepress.authorsSarah Clifford
avondale-bepress.authorsMarcel Maeder
avondale-bepress.authorsGraeme Puxty
avondale-bepress.context-key12530204
avondale-bepress.coverpage-urlhttps://research.avondale.edu.au/sci_math_papers/95
avondale-bepress.document-typearticle
avondale-bepress.field.author_faculty_disciplineScience
avondale-bepress.field.avon_earlyonline2018-06-26T00:00:00-07:00
avondale-bepress.field.comments<p>Due to copyright restrictions this article is unavailable for download.</p> <p>Copyright © 2018 American Chemical Society</p> <p>At the time of writing Sarah Clifford was affiliated with the University of Newcastle.</p>
avondale-bepress.field.custom_citation<p>Li, L., Bennett, R., Conway, W. O., Yu, H., Clifford, S., Maeder, M., & Puxty, G. (2018).<strong> </strong>Development and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-based CO2 and SO32- and SO42- Loaded Capture Process<em> </em>Solutions via FT-IR Spectroscopy.<em> Energy & Fuels, 32</em>(8), 8563-8570. doi:10.1021/acs.energyfuels.8b00762</p>
avondale-bepress.field.doihttps://doi.org/10.1021/acs.energyfuels.8b00762
avondale-bepress.field.email_boxtrue
avondale-bepress.field.embargo_date2018-07-23T00:00:00Z
avondale-bepress.field.field_of_education01 Natural and Physical Sciences
avondale-bepress.field.for03 CHEMICAL SCIENCES
avondale-bepress.field.issn1520-5029
avondale-bepress.field.issue_number8
avondale-bepress.field.journalEnergy & Fuels
avondale-bepress.field.page_numbers8563-8570
avondale-bepress.field.peer_reviewBefore publication
avondale-bepress.field.publication_date2018-08-18T00:00:00Z
avondale-bepress.field.source_fulltext_urlhttps://doi.org/10.1021/acs.energyfuels.8b00762
avondale-bepress.field.source_publication<p>This article was originally published as:</p> <p>Li, L., Bennett, R., Conway, W O., Yu, H., Clifford, S., Maeder, M., & Puxty, G. (2018).<strong> </strong>Development and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-based CO2 and SO32- and SO42- Loaded Capture Process<em> </em>Solutions via FT-IR Spectroscopy.<em> Energy & Fuels, 32</em>(8), 8563-8570. doi:10.1021/acs.energyfuels.8b00762</p> <p>ISSN: 1520-5029<em><br /></em></p>
avondale-bepress.field.staff_classificationContract
avondale-bepress.field.volume_number32
avondale-bepress.keywordsemissions reductions
avondale-bepress.keywordsenergy production
avondale-bepress.keywordschemistry
avondale-bepress.label95
avondale-bepress.publication-date2018-08-18T00:00:00Z
avondale-bepress.publication-titleScience and Mathematics Papers and Journal Articles
avondale-bepress.statepublished
avondale-bepress.submission-date2018-07-23T19:22:29Z
avondale-bepress.submission-pathsci_math_papers/95
avondale-bepress.titleDevelopment and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-Based CO2 and SO32– and SO42– Loaded Capture Process Solutions via FT-IR Spectroscopy
avondale-bepress.typearticle
dc.contributor.authorPuxty, Graeme
dc.contributor.authorMaeder, Marcel
dc.contributor.authorClifford, Sarah
dc.contributor.authorYu, Hai
dc.contributor.authorConway, William
dc.contributor.authorBennett, Robert
dc.contributor.authorLi, Lichun
dc.date.accessioned2023-11-01T00:27:03Z
dc.date.available2023-11-01T00:27:03Z
dc.date.issued2018-08-18
dc.date.submitted2018-07-23T19:22:29Z
dc.description.abstract<p>CO<sub>2</sub> capture using aqueous ammonia is a potentially attractive option for emissions reductions from energy production and industrial processes. From an operational perspective, the capture absorbent must be monitored continuously to maintain the maximum efficiency of the capture process. In practice the composition of the absorbent is typically evaluated offline and retrospectively via wet chemistry methods, delaying any necessary variations to the process conditions to maintain maximum efficiency. Online absorbent monitoring methods incorporating spectroscopy via Raman or Fourier transform infrared (FT-IR) are attractive options due to their rapid response times and flexibility of the resulting output to be incorporated directly into process control packages. The present study outlines an evaluation of the FT-IR spectroscopic technique with analysis via partial least squares regression (PLSR) for a range of dilute to concentrated aqueous ammonia absorbents from ∼0.3–6.0 M and over a range of CO<sub>2</sub> loadings from ∼0.0–0.6 mol CO<sub>2</sub>/mol NH<sub>3</sub>. The water concentration in the samples ranges from ∼35.2–55.2 M. The effect of interfering SO<sub><em>x</em></sub> species on the FT-IR method has been evaluated by incorporating dissolved SO<sub>3</sub><sup>2–</sup> and SO<sub>4</sub><sup>2–</sup> components into the solutions from 0.0–1.5 M. The analysis results in accurate concentrations for all analytes. The robustness of the analysis results has been evaluated and discussed. Additionally, FT-IR spectroscopy with PLSR was compared with conventional titration methods for a selected series of mixed NH<sub>3</sub>/CO<sub>2</sub> standard solutions and a series of liquid samples from a bench-scale CO<sub>2</sub> absorption process. At low concentrations where the total NH<sub>3</sub> concentration is less than 4.0 M and the total CO<sub>2</sub> concentration is less than 1.5 M, both the combined PLSR with FT-IR method and the conventional potentiometric titration methods were suitable for the evaluation of the liquid compositions. However, at concentrations out of the low concentration range, the combined PLSR and FT-IR method was proven to have a robustness and accuracy greater than those of the conventional potentiometric titration methods. Therefore, given the simplicity and rapid turnaround of FT-IR spectroscopy in combination with PLSR, we consider this to be a superior and flexible technique for monitoring of CO<sub>2</sub> loaded aqueous ammonia solutions.</p>
dc.description.versionBefore publication
dc.identifier.citation<p>Li, L., Bennett, R., Conway, W. O., Yu, H., Clifford, S., Maeder, M., & Puxty, G. (2018).<strong> </strong>Development and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-based CO2 and SO32- and SO42- Loaded Capture Process<em> </em>Solutions via FT-IR Spectroscopy.<em> Energy & Fuels, 32</em>(8), 8563-8570. doi:10.1021/acs.energyfuels.8b00762</p>
dc.identifier.doihttps://doi.org/10.1021/acs.energyfuels.8b00762
dc.identifier.issn1520-5029
dc.identifier.urihttps://research.avondale.edu.au/handle/123456789/12530204
dc.language.isoen_us
dc.provenance<p>This article was originally published as:</p> <p>Li, L., Bennett, R., Conway, W O., Yu, H., Clifford, S., Maeder, M., & Puxty, G. (2018).<strong> </strong>Development and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-based CO2 and SO32- and SO42- Loaded Capture Process<em> </em>Solutions via FT-IR Spectroscopy.<em> Energy & Fuels, 32</em>(8), 8563-8570. doi:10.1021/acs.energyfuels.8b00762</p> <p>ISSN: 1520-5029<em><br /></em></p>
dc.rights<p>Due to copyright restrictions this article is unavailable for download.</p> <p>Copyright © 2018 American Chemical Society</p> <p>At the time of writing Sarah Clifford was affiliated with the University of Newcastle.</p>
dc.subjectemissions reductions
dc.subjectenergy production
dc.subjectchemistry
dc.titleDevelopment and Evaluation of a Novel Method for Determining Absorbent Composition in Aqueous Ammonia-Based CO2 and SO32– and SO42– Loaded Capture Process Solutions via FT-IR Spectroscopy
dc.typeJournal Article
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